Process for the separation of gaseous mixtures into their elements.



G. CLAUDE & R. J. LEVY. PROGESS FOR THE SEPARATION OF GASEOUS MIXTURES INTO THEIR ELEMENTS.

APTLIOATION TILED JUNE 3, 1904.

967,105. Patented Aug. 9,1910.

witnesses @af Q47 anvawtoza To all whom it may concern:

UNITED STATES PATENT'oE-FIOE eEoReEscLAUnE, or NoeEE'r sUR-maRNEQ-mwn ENE JadouEs ma or EouLOeNE- suR-sEmE, FRANCE, AssIeNo s T0 SOGIETE L'AIR IQUIEE (sOcIE'rE 'ANONYMZE POUR, LE'IUDE E'l L'ExrLOma'rIOu nEs rROcEnEs GEORGES CLAUDE), or PARIs r AEcE.

1 RocEss FOR THE SEPARATION oEcAsEoUs MIXTURES mo THEIR Enmn'rs.

Specification of letters latent.

PatentedAiug. 9, 1910. I

1 Application filed June a, 1904. Serial E0. 210,937.

Be it known that We, GEORGES CLAUDE, a

-citizen of France, and resident'of Nogentsur-Marne, Department of the Seine, France, and RENE JAC UES LEVY, a citizenof France, and resident of Boulogne-sur-Seine, France, have invented an Improved Process for the Separation of Gaseous Mixtures into Their Elements, for which we have. obtainedLet-" ters Patent of thewRepublic of'France, No. 338,842, dated June 3, 190.3, and of which the following is a specification. v

Although our invention has a wide appli cation for the separation of gaseous mixtures of every kind and proportion into their elements, we shall describe it more particularly as a new process for the separation of oxygen in any desired degree'of purity from atmospheric air by means of evaporation and liquefaction. I, I

This process is based upon the fact ascertained by us that in order to transform liquid air into very pure liquid oxygen by the progressive evaporation of the nitrogen and the simultaneous liquefaction of a, corresponding quantity of oxygen, it issufiicient'to bring nearly pure cold gaseous oxygen into contact with liquid air 1n any manner, as for instance bycausing the gaseous oxygen to pass in bubbles-through the liquid air; By evape orating the liquid oxygen which is obtained we obtain a quantit of gaseous oxygen.

greater than that use ,and if the apparatus 1s suit-ably devised, greater than the quantity of oxygen previously contained in the liquid air used, and this'entire excess may be furnished by the atmosphere. This evaporation of the oxygenis made use of in our inven tion. It is efiected by forcing cold air under suitable pressure into a tubular vesselor into a coil immersed in liquid oxygen. The evaporation of oxygen will thus cause the condensation of a substantially equivalent quantity of air underpressure, and we thus obtain a quantity of liquidair nearly equal. .to that at the start whichin its turn is sepae rated into pure oxygen by repeatingv the same V operations.

the simple passage .in' bubbles through liquid mass would yield poor results, for itis In order to give this method itshighest.

practical value, it is essential that the oxy; gen'gas be utilized as completely as poss1ble;;

the

- evident that the gas at its outcome from ,the liquid holding a large quantity of oxygen would itself contain very'much oxygen and" the loss would be greater thanthe gain. It

is therefore of importance that-this passage 7 of theoxygen gas through the liquid air be carried out in a particular manner, for into stance, by supplying the liquid air to be converted into oxygen at the up er part of an. column-provided with baflle ates or other suitable device and by su plying the gaseous oxygen at the lower en of the column, so that the gas travels'throu h the successive chambers and issues from t e column at the point of sup 1y of the liquid air;

It is well licnown that if the liquid air at its formation contains like the "atmospheric air about 21 per cent. of oxygen, the gas at its issue contains only about 6 or 7v per cent.

. of oxygen. If it be necessary to retain these quantities, it is possible to provide the column with an extension at the end ofwhich we feed liquid air containin less than 21" per cent-of oxygen obtained, tor instance, in the manner described in the pending appllcation for Letters Patent of the United J States No. 187,307, filed December 31st 1903 by Georges Claude one of these applicants.

The losses in cold in the column can be compensated for either by the introduction of iquid air obtained from an auxiliary source, j or by' the ex ansion of the air to be liquefied, com ressed or this object to a higher degree.

T e drawin shows anove apparatus which. we have invented to carry our method .into'efiect. .7 i" In this figure A is an insulated metalllc c lindr carryin in its upper partthe perfh rated plates p p, the lower part of whichv is provided with a partition 0 f0 ing a" chamberkM communicating with the upper art N'of the cylinder by means of'a pipe descending: into the lowei' part, In- M 1s containeda coil S with feed aperture t, and which extends into a tube T provided with a cock R paminginto the up or part of the cylinder-and ending above t e top plate 10 The gas evaporated in M distributes itse f through thepipes t and t of vvhich'the pipe t". is perforated and is situated [below the lower perforated plate of chamber M and the ipe t leads to the exterior through interc angers used in, this kind of apparatus,

through which the vapor circulates in a direction opposite to that of the air pr gas to be separated.

It will be noted that during the ascension 0f the vapbr up the part N, the vapors becoming progressively poorer in oxygen, will at a certain height present the com osition ,;of the atmospheric air. If'at this p ace atmtgspheric air is admitted, its oxygen will be utilized under the same conditions as that of the vapors, and the oxygen thus freely obtained from the atmosphere increases the quantity'of oxygen obtained and thus 'increases the economic value of the process;

the more so because it is not necessary to compress such air and it will be suflicient to cool thesame in an interchanger by means I of the counter current of some of the cold gas emanating fromthe apparatus. It is to e remarked that by this introduction of air,

To start the apparatus a quantity of'liquid air sufiicient to cover the coils S of the chamber M is introduced, then gaseousair is in-' troduced into the coil S havlng in relation to the exterior liquid a sufiicient excess of pressure -to bring about its liquefaction. The

gas

' rection opposite to the product of this liquefaction is passed to the topof theapparatus through T, the flow being regulate by the cock R. The liquid runs downward from plate to plate in a diaseous flow'which starts from axpart'of t e products of the evaporation in M emanating through if in art of N; the balance of the.

the lower products 0 evaporation passes out through apparatus for the separation 0 mixed gases t, and circulates in a direction opposite 'to that of the air or gas to .be separated. The liquid flowing downward in the apparatus becomes progressively richer in oxygen and finally on y pure oxygen evaporates in M, of which the part not utilized in the cylinder is collected at the exterior and is utilized.

It is, of course, necessary in practice to regulate very precisely the counter pressures of the interchangers through which the different gases travel soas to obtain the complete equality of pres'sure in M and N, which 1s necessary in order'to cause the liquid to flow readily from N into M. In the liquid a1r or li uid mixtures of oxygen and nitrogen we t us increase progressivel the quantlty of oxy en contained therein y the substltution .o the nitro en of the liquid by the gaseous oxygen, the liquid oxy en thus obtained being in turn evapora in liquefying another portion of air or of the mixtures to be separated.

We may employ the foregoin process and other than oxygen and nitrogen into their elements'and we do not confine our claims to the separation of atmospheric air or to v the separation of any particular mixture of gases into, tlieir elements.

'What we claim and desire to secure by Letters Patent of the-United States is 1'. A process for separating atmospheric air into. its constituents, which consists in compressing, cooling, and liquefying the air, subjectmg the liquefied part or parts to rectification, collecting in a single com artment the liquid oxygen or liquid ric in oxygen resulting from the rectification, completely vaporizm in this single compartment the aforesai liquid by circulatin the whole of the cpld compressed air in in 'irect contact with it, causing the liquid resulting from the aforesaid circulation and consequent liquefaction of the cold compressed air to descend through a rectifier into the aforesaid single compartment, eifecting a direct withdrawal from above the surface of the liquid there'in of a ortion of the vapors rising from said liqui and conducting the remainder only of the vaporsin the opposite direction-to'and incontactwith the escendin llqllxlld to progressively enrich it in oxygen y t e substitution of the oxygen of the vapors for the nitrogen, of the liquid, no liquid being withdrawn from the single compartment.

2. A process for separating atmospheric air into its constituents which consists in passing cold compressed air through but not in direct contact with the liquid oxygen or liquid rich in oxygen which results from the separation and is thereby vaporized, 'causlng the liquid resulting from the said liquefyin of the cold compressed air to flow downwar 'in the opposite direction to and in contact with the vapors ascending from the 11 uidoxlyigen or liquid rich in oxygen, and ad ing co gaseous a1r to the ascending vapors at a point where they are of approxlmately atmospheric composition.

3. A process for separating atmospheric air into its constituents, which consists in liquefying cold compressed air in a yaporizing com artment containing the liquid ox gen or uid rich in oxygen which resu ts fromv t e separation, and is thereby vaporized, causing the 1iqu1d resulting from the said liquef ing of the cold com ressed air to descend y stages into the sai vaporizing compartment, conducting art of the vapors ascending therefrom in t e opposite direction to and 1n contact with the descending liquid to rogressivel enrich it in oxygen by the su stitution o the ox gen of the -va ore for the nitrogen of the iquid', and adding cold gaseous air to the ascending vapors at a pomt where they are of'approximatelX atmospheric composition.

process for separating atmospheric samba liquefying cold compressed air in a va or1z- I and nitrogen, poorer in oxygen than the l ing com artment containing the liqui oxyen or iquid rich in oxygen which results rom the separation, and is thereby vaporized, causing the liquid resulting from the said liquef ing of the cold compressed air to descend y stages into the said vaporizing compartment, conducting art of the vapors ascending therefromv in t e opposite direction to and in contact with the descending liquid to progressively enrich it in oxygen, by the substitution of the oxygen 'of the va ors for the nitrogen of the l' uid, and ad ing a cold gaseous mixture 0 oxygen vapors immediately abovethe liquid in the vaporizing compartment, to the ascending vapors, at a point where they are of approximately the-same composition as the aforesaid gaseous mixture, and at a pressure only sufiicient to enable it to ascend, together with the aforesaid vapors, through the des'cending liquid. 1

In witness whereof, we have hereunto set our hands atParis, France, this twenty-first day of May 1904.

GEORGES CLAUDE. RENE JACQUES LEVY. In presence of-. i HANSON O. Goxn, CHARLES OHAPUIS. 

